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international journal of hydrogen energy xxx (xxxx) xxx

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Co-gasification between coal/sawdust and coal/


wood pellet: A parametric study using response
surface methodology

Fatin Zafirah Mansur a, Che Ku Mohammad Faizal a,*,


Minhaj Uddin Monir a,b, Nur Asma Fazli Abdul Samad c,
Samson Mekbib Atnaw d, Shaharin Anwar Sulaiman e
a
Faculty of Engineering Technology, University Malaysia Pahang, 26300 Gambang, Pahang, Malaysia
b
Department of Petroleum and Mining Engineering, Jessore University of Science and Technology, Jessore, 7408,
Bangladesh
c
Faculty of Chemical and Natural Resources Engineering, University Malaysia Pahang, 26300 Gambang, Pahang,
Malaysia
d
College of Electrical and Mechanical Engineering, Addis Ababa Science and Technology University, Ethiopia
e
Department of Mechanical Engineering, Universiti Teknologi Petronas, 32610 Bandar Seri Iskandar, Perak,
Malaysia

highlights graphical abstract

 Co-gasification performance on
raw biomass and pre-treated
biomass with coal.
 Effect of operating variables on the
performance parameters are stud-
ied using RSM.
 Experimental results are in good
agreement with the predicted
values.
 The optimum H2/CO ratio and
HHVsyngas are found at high ER for
both co-gasification.

article info abstract

Article history: This study had compared raw biomass and pre-treated biomass co-gasified with coal with
Received 24 September 2019 the aim of investigating the reliability of pre-treated biomass for enhancing gasification
Received in revised form performance. Sawdust (SD) and wood pellet (palletisation form of sawdust - WP) and
2 March 2020 blends of these two feedstocks with sub-bituminous coal (CL), were gasified in an air at-
Accepted 5 April 2020 mosphere using an external heated fixed-bed downdraft gasifier system. Response surface
Available online xxx methodology (RSM) incorporating the central composite design (CCD) was applied to assist

* Corresponding author.
E-mail address: mfaizal@ump.edu.my (C.K.M. Faizal).
https://doi.org/10.1016/j.ijhydene.2020.04.029
0360-3199/© 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
2 international journal of hydrogen energy xxx (xxxx) xxx

Keywords: the comparison of all operating variables. The three independent variables were investi-

Co-gasification gated within a specific range of coal blending ratios from 25% to 75%, gasification tem-

Coal perature from 650 C to 850  C and equivalence ratio from 0.20 to 0.30 against the

Sawdust dependent variables, namely the H2/CO ratio and higher heating value of the syngas

Wood pellet (HHVsyngas). The results revealed the H2/CO ratio and a higher heating value of the syngas

RSM of more than 1.585 and 6.072 MJ/Nm3, respectively. Findings also showed that the H2/CO
ratio in the syngas from CL/WP possessed a higher value than the CL/SD. In contrast, CL/SD
possessed a higher heating value for syngas with about 1% difference compared to the CL/
WP. Therefore, co-gasified coal with wood pellets could potentially be a substitute for
sawdust.
© 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

respectively, compared to raw switchgrass [11]. The analysis


Introduction by Ref. [11] also revealed that pelletized switchgrass exhibits a
severely disintegrated fibrous structure, whereas the fibrous
Overconsumption of fossil fuel due to global energy demands matrix in the unpelletized switchgrass was still visible. These
has dramatically increased over the past several decades as a deviations have led to efficient performances during gasifi-
consequence of the advancement in industrial fields and cation. Co-gasification of garden waste pellets with Indian
improvement in the living standards on a worldwide scale coal shows an increase in biomass ratio resulting in the
resulting in the scarcity of energy sources [1]. Biomass is highest production of H2 and CO with the lowest heating value
viewed as a carbon-neutral form of energy that provides a of 3.05 MJ/Nm3 [13]. Furthermore, co-gasification’s modelling
significant source of renewable energy [2]. The addition of a of coal with wood pellet revealed that the CO concentration
high calorific value and presence of an appropriate catalyst decreased and H2 increased with the increase in the blend
(coal) into the biomass provides a heat source for biomass ratio. For the gasification performance, carbon conversion and
gasification, which enhances the reaction rate and stabilises cold gas efficiencies for all blend ratios were more than 99.8%
the gasification process [3,4]. Thus, utilizing biomass and coal and 88.1%, respectively [14]. However, to the best of our
has been a passage between renewable and non-renewable knowledge, few conclusions have been drawn between the co-
resource-based energy production, especially in co- gasification of coal with raw biomass or pre-treated biomass,
gasification [5,6]. Raw biomass with a high moisture content with either possessing better gasification performance with
and low energy density together with high transportation similar parameters. Considering these factors, a comprehen-
costs hinders its application in the corresponding gasification sive investigation on the optimization of raw biomass and
process [7,8]. On the improvement of biomass properties, pre-treated biomass for co-gasification with sub-bituminous
various pre-treatment methods have been developed to coal should be performed by applying the response surface
enhance its implementation. Densification is a solution to methodology (RSM) with various responses and outputs.
tackle low-density technical issues. Gasification of pellet fuel Response surface methodology (RSM) is an effective
is widely applied in commercial gasification resulting in a statistical tool for research purposes, which employs both
stable syngas composition by maintaining a steady and effi- statistical and mathematical methods to develop, improve
cient gasification process. The uniform shape and density of and optimize the process, as well as to investigate several
the pellet fuel aids in smooth feeding by making less biomass important responses affected by some variables [15].
bridges and gasification reactions [9]. Due to these merits, There are many downdraft gasifiers developed worldwide
pelletized biomass is frequently applied in gasification, espe- for co-gasification; unfortunately, very few studies have
cially in fixed-bed gasifiers, where mechanically, substantial been done on the prediction of the gasification perfor-
fuel particles of limited size are required for successful oper- mance and incorporate process parameters, like coal
ations [10]. Thus far, only several studies have explored the blending ratio, temperature and equivalence ratio. More-
gasification performance of pelletized biomass with its parent over, there are no studies on RSM related to pre-treated
biomass [11,12]. Yoon conducted the downdraft fixed-bed biomass, especially with coal or comparative studies on
gasifier using rice husk and rice husk pellets and found that RSM using raw biomass or pre-treated biomass with sub-
rice husk pellets produced a better syngas composition of bituminous coal.
18.6%, 20.2%, 8.1%, and 1.5% for H2, CO, CO2, and CH4, In the present study, the physical and chemical properties
respectively. In addition, the higher gas value and cold gas of sub-bituminous coal (CL), raw biomass-sawdust (SD) and
efficiency of the rice husk pellet increased significantly (15%) pre-treated biomass-wood pellet (WP) were investigated to
compared to raw rice husk. Densified switchgrass also resul- determine the characteristic of each feedstock for corre-
ted in better gasification performance at 4.46 MJ/m3, 89.58% sponding co-gasification investigations. Furthermore, the co-
and 63.98% for lower heating value (LHV) of syngas, carbon gasification of biomass with a blend of different coal
conversion efficiency (CCE) and cold gas efficiency (CGE), blending ratios, gasification temperature and equivalence

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
international journal of hydrogen energy xxx (xxxx) xxx 3

Fig. 1 e Images of coal, CL (a), sawdust, SD (b) and wood pellet, WP (WP) that were used throughout this study.

ratios has been investigated in an externally heated down- Co-gasification experiment


draft fixed-bed gasifier system. The H2/CO ratio in the syngas
and the higher heating value of the syngas (HHVsyngas) were The co-gasification of CL/SD and CL/WP was carried out in a
obtained through a series of experimental investigations. A fixed bed downdraft gasifier located at the biomass laboratory,
central composite design (CCD) incorporating the RSM under Department of Mechanical Engineering in Universiti
method was applied to reveal the effects of interaction be- Teknologi Petronas (UTP), Perak. The schematic diagram for
tween several operating variables. The results indicate that the complete gasifier system comprising three main compo-
the models developed through the Design Expert 10 fit nents, namely the gasifier reactor, gas cooling associated with
agreeably with the experimental results for all the response the cleaning system and the online gas analyser, is shown in
variables involved. Fig. 2. The gasifier was operated at atmospheric conditions of
1e2 h for each experiment. Air, used as a gasifying agent, was
supplied to the gasifier using a 1.5 kW air compressor at a
Methodology pressure of 2 bar. Meanwhile, the rotameter, which monitors
air flow control, was attached to the gasifier system. The in-
Feedstock preparation and analysis ternal diameter and height of the gasifier were 80 mm and
500 mm, respectively. Besides, an electric furnace enclosed
The CL/SD and CL/WP blends were used as feedstock in this around the reactor mainly functioned to heat the gasifier. The
study. The CL was obtained from an electric utility company in gasifier was then flushed with compressed air at the required
Malaysia through a third-party company. Meanwhile, the SD amount of volume (0.12e0.24 Nm3/h) for 10 min before the
and WP were obtained from a wood industry company located experiment to achieve a stable state. Subsequently, the
in Penang, north of Malaysia. Both SD and WP are recognized reactor was heated to the desired gasification temperature.
as the by-product of woodworking operations and pre-treated Once the reactor achieved a stable state with the desired
sawdust in a pelletized form. Fig. 1 shows the images of CL, SD
and WP. Both CL and SD were received in powder form, while
WP was in solid form. The dimensions of the feedstock were
determined by using the Brunauer-Emmett-Teller (BET) the-
ory and the Malvern particle sizer model. The feedstock was
received prior to the day of the experiment from a local sup-
plier. The feedstock was prepared for investigating the
texture, structure and chemical properties of CL, SD and WP as
well as corresponding co-gasification experiments. Samples
were first weighed to obtain the required mass needed
throughout the experiment. Next, samples were dried in an
oven at a temperature of 105  C for about 24 h. The main
purpose of the drying process was aimed at removing most of
the moisture in the samples. Subsequently, samples were
mechanically mixed into different blending ratios (25%, 50%,
and 75%). Then, the dried samples were placed into an air-
tight container to avoid any moisture coming in contact
with the samples. The properties of the feedstocks were
determined by a proximate analysis as per the ASTME1131 [16]
procedure using a thermogravimetric analyser (Hitachi STA
7000), ultimate analysis as per the ASTM D3176 [17] procedure
using an elemental analyser (Elementar: vario MACRO cube),
and higher heating value (HHV) using a bomb calorimeter (IKA
Fig. 2 e The schematic diagram of the external heated
C200).
fixed-bed downdraft gasifier system.

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
4 international journal of hydrogen energy xxx (xxxx) xxx

gasification temperature and air flow rate, a sample weighing the CO, CH4 and H2 obtained from online gas analyser mea-
approximately 100 g was loaded into the gasifier reactor by surements where each was multiplied by its respective HHV,
applying the drop-chute method. Produce gas was let into the and the sum of the multiplication products represent
gas analysis unit. The gas analysis was carried out until all the HHVsyngas. The HHV for each gas was 12.63 MJ/Nm3 for CO,
samples were fully consumed, which was for about 20 min, 39.82 MJ/Nm3 for CH4 and 12.74 MJ/Nm3 for H2 as per standard
and the gaseous composition displayed negative values. Once value obtained from the US National Renewable Energy Lab-
the process was completed, the electric furnace and air oratory (NREL) [19].
compressor was switched off and the gasifier was left to cool.
The solid residue, which was characterized as char from the Design of the experiment
experiment, was collected from the gasifier at the bottom
opening. The final weight of the remaining char was then An empirical modelling approach known as Response Surface
weighed using a precision weight balance once it reached Methodology (RSM) was chosen as the experimental design
room temperature. The temperature and gas composition using the Design Expert software (Version 10.0.3, Stat-Ease
readings from the experiment were obtained from a desktop Inc., MN, USA). In this study, the selected factors were opti-
computer for analysis purposes. mized by applying the centre composite design (CCD) in RSM.
From the value of the gaseous product obtained from the Generally, CCD is one of the conventional designs existing in
gas analysis unit, the H2/CO ratio in the syngas was defined as RSM. CCD incorporates two-level full or fractional factorial
one of the response variables. It was an essential parameter to designs with the addition of axial points consisting of at least
study as a product of the gasification that produces syngas (H2 one point at the centre of the experimental range. The CCD is
and CO) for the chemical synthesis (e.g. methanol, liquid fuels also an alternative to the full factorial three-level design since
or for the Fischer-Tropsch process) that generates energy [18]. it requires lesser number of runs instead of the stipulated
Moreover, the higher heating value of the syngas (HHVsyngas) corresponding outcomes [20]. Three operating variables
was calculated. It was a crucial output parameter that defines involved in this study were the coal blending ratio (A), gasifi-
the quality of syngas produced from gasification in terms of cation temperature (B) and equivalence ratio (C). Meanwhile,
energy content per unit volume or mass. The higher heating the range of variables considered were coal blending ratio
value of syngas (HHVsyngas) was calculated by considering the (25e75%), gasification temperature (650e850  C), and equiva-
percentage volume of combustible gas components in the lence ratio (0.2e0.3). Equally important is the determination of
syngas (CO, H2 and CH4) produced from the co-gasification the higher and lower boundaries for the input variables in
experiment with a specific HHV, expressed in the following regards to the preliminary results and experimental setup
Eq. (1). limitations. Meanwhile, the H2/CO ratio of syngas and the
  higher heating value of syngas (HHVsyngas) were measured as
HHVsyngas ¼ ðVCO  HHVCO Þ þ ðVCH4  HHVCH4 Þ þ VH2  HHVH2 (1) output variables. In order to evaluate the result, an ANOVA
where, V, is described as the volumetric percentage of each of (analysis of variance) was generated and analysed

Table 1 e Experimental design with output response variables based on the centre composite design (CCD) generated by
Design Expert.
Run Variables Response
Coal/Sawdust (CL/SD) Coal/Wood pellet (CL/WP)
A-Coal (%) B-Temp. ( C) C-ER H2/CO ratio HHVsyngas (MJ/Nm3) H2/CO ratio HHVsyngas (MJ/Nm3)
in syngas in syngas
1 50 750 0.25 1.2723 5.3290 1.1244 5.8600
2 8 750 0.25 0.8900 4.6404 1.2528 3.4806
3 50 582 0.25 0.8681 4.0090 0.8938 3.7667
4 92 750 0.25 0.8477 4.9943 0.9847 4.3032
5 25 850 0.20 0.8864 4.9088 1.4894 5.3054
6 50 750 0.25 1.1874 5.2001 1.1556 5.2806
7 50 750 0.25 1.3693 5.5638 1.1387 5.6480
8 25 650 0.20 0.7810 4.3988 0.7659 4.0170
9 75 850 0.20 0.9357 6.0724 0.7865 4.7907
10 25 850 0.30 0.9271 4.2243 1.6910 3.9759
11 50 750 0.25 1.2202 5.3655 1.1816 5.9161
12 75 650 0.30 0.7344 3.7768 1.3950 4.3527
13 75 850 0.30 1.5837 5.4202 1.4247 4.9239
14 50 750 0.25 1.3736 4.8277 1.1042 6.0160
15 50 750 0.35 0.8758 4.2833 1.4497 3.4323
16 50 918 0.25 1.3332 5.6015 1.3819 5.1468
17 75 650 0.20 0.8026 4.0831 0.8894 3.6235
18 25 650 0.30 0.3796 4.7856 1.0340 3.4405
19 50 750 0.25 1.0726 5.1665 1.0916 5.6321
20 50 750 0.15 0.5838 4.9651 0.7305 4.3937

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
international journal of hydrogen energy xxx (xxxx) xxx 5

Subsequently, the experimental results produced and


Table 2 e The pore size, surface area and dimensions of
calculated were fitted into the model for both co-gasifications
the CL, SD and SDP.
for each response variable. The range of the co-gasification
Sample Pore size (nm) BET (m2/g) Dimensions (mm)
performance for the co-gasification (CL/SD) was 0.380e1.584
CL 4.08 5.71 0.00747 for the H2/CO ratio in the syngas and 3.777e6.072 MJ/Nm3 for
SD 3.77 17.10 0.00362 HHVsyngas; meanwhile, the range for the co-gasification (CL/
WP 4.70 1.35 10e50
WP) was 0.731e1.691 for the H2/CO ratio in the syngas and
3.432e6.016 MJ/Nm3 for HHVsyngas. Range of the co-
gasification performance obtained from other co-
gasifications using CL and SD as fuel indicates a difference
numerically. It is capable of analysing the interaction and
of about 20% recorded from 1.6 to 4.4 MJ/Nm3 [22], which was
individual influence of independent variables on dependent
carried out in a fluidized bed gasifier. Commonly, the high
variables. Subsequently, the regression model, significance of
value of HHVsyngas in this study might be due to the applica-
terms and lack-of-fit tests were carried out to assess the
tion of the downdraft gasifier that leads to minimising the
goodness of fit, which indicates whether the proposed models
generation of tar content and eventually enhancing the gasi-
are a statistically significant. These were subjected to the
fication performance [23]. On the other hand, the range of the
probability value (p-value) with a confidence level of 95%.
H2/CO ratio in the syngas for the co-gasification of CL and WP
Meanwhile, the precision of experimental data from the
were found to be slightly similar, such as from 0.77 to 1.52 [24].
model was determined based on the value of the regression
coefficient (R2). Since the regression coefficient was at l (within
the range of 0e1) or with the value being closer to 1, it shows
Results and discussions
that the model can provide a good prediction for the output
variables [21]. Furthermore, the interaction of factors together
Characteristics of the feedstock
with their outcomes on the response is presented in the form
of three-dimensional graphs. This graphical information was
Table 2 provides the pore structure parameters as well as the
used to simultaneously interpolate the combination of in-
surface area and dimensions of CL, SD and WP, with SD hav-
teractions to intermediate points, which are difficult to study
ing the least pore size compared to CL and WP. Meanwhile, the
experimentally.
surface area of SD is higher than WP and CL. This denotes that
Table 1 presents a full design matrix generated comple-
the higher surface area is supportive of an increase in gasifi-
mentary to the CCD design, in which the experiment was
cation reactivities [25]. In addition, the powder dimensions of
conducted based on it. A total of 20 runs were designed
CL and SD were determined. The results are consistent with
comprising eight factorial points, six axial points and six
the surface area and dimension in which the smaller di-
replicates at the centre point. In this study, the experimental
mensions of the feedstock possess a higher surface area with
run was randomized to reduce the error and effect of uncon-
less pore size.
trolled factors. The experimental data were collected to
Results of the proximate analysis, ultimate analysis and
generate the empirical second-order polynomial equation
calorific analysis (as shown in Table 3), as well as SEM mi-
employed as shown in Eq. (2).
crographs, provide some important insights regarding the
X
k X
k X
k X
k chemical and structural properties of each feedstock. Based
Y ¼ b0 þ bi xi þ bii x2ii þ bij xi xj þ ε (2) on the proximate analysis of the sample, CL contained a low
i¼1 i¼1 i¼1 j¼iþ1
percentage of MC, VM, and FC as compared to SD and WP. The
where, Y is the predicted response, b0 is the intercept, bi is the proximate analysis’s value of each CL, SD and WP are in the
linear coefficients, bii is the quadratic coefficient, and bij is the range of data marked by other researchers [26,27]. It is ex-
interaction coefficients for both variables i and j. Meanwhile, ε pected that CL has the highest gasification efficiency; how-
is referred to as the random error. ever, it has a disadvantage on the latter in the form of risks,

Table 3 e Proximate, ultimate and higher heating value of coal/sawdust and coal/wood pellet.
Samples Proximate analysis (wt. %) Ultimate analysis (wt. %) HHV (MJ/kg)
MCa VMb FCc Ash C H N S Od
100% CL 8.18 39.79 33.81 18.22 52.58 5.90 1.49 1.14 38.90 20.19 ± 0.082
100% SD 11.8 68.05 19.05 1.10 44.11 5.53 2.14 2.70 45.52 17.17 ± 0.089
100% WP 9.19 79.00 10.16 1.65 44.28 6.09 1.05 0.28 48.62 17.46 ± 0.085
Blend of coal & sawdust 75CL/25SD 12.27 47.89 36.65 3.19 50.46 5.80 1.65 40.55 1.53 18.04 ± 0.206
50CL/50SD 10.92 48.23 38.41 2.44 48.35 5.71 1.82 42.21 1.92 18.75 ± 0.099
25CL/75SD 9.65 56.86 31.35 2.14 46.23 5.62 1.98 43.86 2.31 17.94 ± 0.084
Blend of coal & wood pellet 75CL/25WP 9.92 80.85 6.38 2.85 50.50 5.86 1.38 41.33 0.92 19.00 ± 0.389
50CL/50WP 9.32 79.13 8.83 2.72 48.43 5.83 1.27 43.76 0.71 18.28 ± 0.641
25CL/75WP 9.44 80.74 7.14 2.68 46.36 5.79 1.16 46.19 0.50 18.12 ± 0.112

Moisture contenta, Volatile matterb, Fixed carbonc, By difference: Od¼ (100 - (Cþ H þ N þ S)).

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
6 international journal of hydrogen energy xxx (xxxx) xxx

the thermal pre-treatment process that applied densification.


It can also be observed that the blend of sawdust with coal is
located a bit farther from its parent material, namely SD. It is
expected that the addition of CL into sawdust will result in
changes in characteristics of the SD itself due to synergism
[31]. Besides, the result indicates that the selected biomass
transformed into a highly volatile matter (>70%) and the FC
contents acted as favourable properties for the gasification
process [29].
In addition, the morphology of the main feedstock was
investigated by employing the Scanning Electron Microscope

Fig. 3 e Ternary diagram based on the value of VM, FC, and


AC for CL, SD, WP and its blends.

such as clogging, slagging and fouling due to high amounts of


ash compared to biomass [19]. Therefore, co-gasified CL with
SD and WP might reduce this disadvantage and result in
greater gasification efficiency. In addition, as clearly expected,
MC in WP (9.19%) reduced by 11.80% (SD) due to the thermal
pre-treatment process in densification, which it was subjected
to during the manufacturing process [9]. Moreover, the VM of
the SD and WP are almost twice of the CL, as reported by Refs.
[13]. The blending of CL/WP has the highest percentage of VM
compared to the blending of CL/SD due to blending of CL with
high VM of WP [28]. According to the difference in terms of FC,
SD/CL’s blending possesses the highest FC compared to WP/
CL due to the high percentage of FC in SD. Considering the
physical and chemical properties of the feedstock, the perti-
nence of solid fuel for thermal conversion purpose can be
foreseen by locating it on a ternary diagram, which has been
recognized as a ubiquitous approach for many years [29].
Meanwhile, from the ultimate analysis, the C content in CL is
much higher (52.58%) than SD and WP, with 44.11% and
44.28%, respectively, which might result in a high composition
of carbon-monoxide in syngas [30]. Another essential point is
that WP has a much lower N and S content than CL and SD
resulting in the least possibility of NOx and SOx generated
during the downdraft gasification process. One significant
note is that the SD in this study possessed a higher S content
compared to CL, which might cause corrosion to the metallic
parts of the gasification equipment and make syngas unde-
sirable for methanol synthesis. One evident point is the
decreasing order of HHV from CL ˃ WP ˃ SD. The amount of
HHV for each CL, SD and WP were also in the range mentioned
by other researchers [14,22]. Subsequently, HHV for all the
blending fuel ratios was between 19.00 and 17.94 MJ/kg.
Furthermore, as expected, an increase in the blends of CL with
SD and WP resulted in an increase in the feedstock’s HHV
value.
The ternary diagram in Fig. 3 also presents a summary of
the blending ratio for each CL/SD and CL/WP. It shows that SD
and WP are close to each other as both come from the same Fig. 4 e SEM Image of (a), (b), (c) are CL, SD and WP,
source, while WP is in a pelletized form as it has undergone respectively at a magnification of 2000x.

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
international journal of hydrogen energy xxx (xxxx) xxx 7

Table 4 e Analysis of variance (ANOVA) for co-gasification of CL/SD and CL/WP.


Source Coal/Sawdust (CL/SD) Coal/Wood pellet
H2/CO ratio HHVsyngas H2/CO HHVsyngas
SS p-value SS p-value SS p-value SS p-value
Model 1.5156 0.0008 6.6468 <0.0001 1.3048 <0.0001 14.8145 <0.0001
A-Coal 0.0750 0.0691 0.1946 0.0508 0.0641 0.0009 0.3992 0.0197
B-Temp 0.4280 0.0007 2.8690 <0.0001 0.3316 <0.0001 2.5347 <0.0001
C-ER 0.0403 0.1663 0.4290 0.0081 0.5822 <0.0001 0.5498 0.0087
AB 0.0136 0.4065 1.6965 <0.0001 0.2641 <0.0001 0.0009 0.8973
AC 0.1105 0.0330 0.0546 0.2672 0.0568 0.0014 0.9579 0.0016
BC 0.1677 0.0123 0.2511 0.0304 0.0005 0.6782 0.2275 0.0629
A2 0.3017 0.0022 0.3904 0.0105 0.0012 0.5462 5.4605 <0.0001
B2 0.0579 0.1038 0.4108 0.0091 0.0035 0.3018 2.5109 <0.0001
C2 0.4754 0.0004 0.6818 0.0020 0.0004 0.7324 5.0062 <0.0001
Residual 0.1808 0.3953 0.0299 0.5196
Lack of Fit 0.1145 0.2815 0.0899 0.8972 0.0244 0.0641 0.1681 0.7812
Pure Error 0.0663 0.3054 0.0055 0.3515
R2 0.8934 0.9439 0.9776 0.9661
Adj R2 0.7975 0.8933 0.9574 0.9356
Pred R2 0.4461 0.8338 0.8504 0.8795

(SEM) model Quanta FEI 450, as shown in Fig. 4. It shows that statistically analysed to evaluate its reliability based on the
the SEM image of CL is composed of a small shiny solid rock- model of the co-gasification experiments using three tests,
like structure. SD illustrates a smooth particle surface; in namely the significance of terms, lack-of-fit and R-squared
contrast, the particle surface of WP is rough and compact. This tests. Table 4 presents the results of both CL/SD and CL/WP
is expected due to the palletisation process in the WP that has with each of the test of significance (on factors) and in-
eliminated the moisture content in the SD and making it drier teractions for three responses. It was discovered that the p-
[9]. value for the whole model determines the significance of the
variables. P-value was less than 0.05, denoting that the indi-
Statistical analysis of the experimental results vidual terms in the model have a significant effect on the
response, and when the p-value is larger than 0.05, the term is
As mentioned earlier, ANOVA is a powerful tool for simulta- insignificant. According to Table 4, the test of significance for
neously investigating several variables instead of only one the effective variables and terms are not similar for different
variable at a time. The repetition at the centre of the design responses. As for the co-gasification of the CL/SD, tempera-
points found in the experimental analysis aids in minimising ture was found to effect the H2/CO ratio in the syngas and the
experimental errors [20]. The result of the ANOVA analysis is coal blending ratio, while the equivalence ratio had influenced
presented in Tables 4 and 5. the HHVsyngas. In contrast, the co-gasification of CL/WP saw all
Table 4 presents the ANOVA (analysis of variance) from the the operating variables affecting the H2/CO ratio in the syngas
co-gasification experiments that aimed to construct empirical and HHVsyngas. Furthermore, the lack-of-fit test was adopted
prediction models generated by the Design Expert. Subse- to determine whether inconsistencies between measured and
quently, the highest order polynomial was selected for each predicted values are associated with random or systematic
model in order to maximize the adjusted R2, where the terms errors. The p-value for lack-of-fit was less than 0.05, denoting
were significant, and the model was not aliased. Therefore, that there is a statistically significant lack-of-fit at the 95%
the quadratic model was chosen for all the operating factors in confidence level. Hence, the p-value for the term “lack of fit” in
the co-gasification of CL/SD and CL/WP, which is significant Table 4, which is greater than 0.05, indicates that the “lack of
for predicting the response variables. Generally, the gasifica- fit” for the whole model for the H2/CO ratio in the syngas and
tion performance for both the SD and WP with CL were HHVsyngas for the co-gasification of both CL/SD and CL/WP is

Table 5 e The empirical correlations were developed based on ANOVA for the co-gasification of CL/SD and CL/WP as a
function of actual and coded operating variables.
Samples Index Type Inter A: Coal B: Temp C: ER AB AC BC A2 B2 C2
Blend of coal & H2/CO Actual 0.83 9.51e-3 3.31e-3 1.670 1.65e-5 0.094 0.029 2.34e-4 6.401e-6 54.169
sawdust Coded 1.25 0.074 0.18 0.050 0.041 0.12 0.14 0.15 0.064 0.14
HHVsyngas Actual 12.50 0.090 0.030 59.04 1.84e-4 0.07 0.035 2.66e-4 1.71e-5 64.870
Coded 5.24 0.12 0.46 0.16 0.46 0.08 0.18 0.17 0.17 0.16
Blend of coal & H2/CO Actual 1.59 0.033 2.40e-3 0.040 7.26e-5 0.067 1.65e-3 1.45e-5 1.59e-6 1.511
wood pellet Coded 1.13 0.069 0.16 0.19 0.18 0.084 8.27e-3 9.03e-3 0.016 3.8e-3
HHVsyngas Actual 37.13 0.04 0.076 95.645 4.27e-6 0.28 0.0337 9.95e-4 4.22e-5 175.78
Coded 5.73 0.17 0.43 0.19 0.011 0.35 0.17 0.62 0.42 0.44

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
8 international journal of hydrogen energy xxx (xxxx) xxx

insignificant. By all means, the model was a fit with the CL/SD and CL/WP were in excess of or close to 80%, denoting
response data collected and necessary for the next experi- that the whole model is regarded as satisfactory when
ments. Meanwhile, the fitness for all models for each response considering the complicated comparative analysis between
variable for the co-gasification of both CL/SD and CL/WP was the co-gasification of SD and WP with CL in the externally
expressed by the R2 value. The R2 for different correlations are heated downdraft fixed-bed gasifier system subjected to at-
provided in Table 4. In brief, the R2 values are close to 1 for all mospheric conditions.
correlations tested, hence, it indicates that all the models are Table 5 demonstrates the functionality of different pa-
of good quality for both co-gasifications. Meanwhile, the rameters to the three operating variables with their in-
adjusted R2 in the regression model for the co-gasification of teractions based on the ANOVA analysis. The actual

Fig. 5 e 3-Dimensional response surface plots representing the combined effect of the coal blending ratio (25e75%),
gasification temperature (650e850  C), ER (0.20e0.30) each for (aec) co-gasification of CL/SD (def) co-gasification of CL/WP on
H2/CO ratio in the syngas.

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
international journal of hydrogen energy xxx (xxxx) xxx 9

coefficients aid in predicting the actual responses using the H2/CO ratio in syngas increased by 26% and 23%, respectively.
original unit. Equally important, the coded coefficients are This is expected due to the increasing value of the H2 con-
suitable for comparing the relative impact of each variable centration and CO gaseous composition from the co-
term on the responses. Table 5 shows that the major influ- gasification of CL/SD and CL/WP. An increase in the gasifica-
encing conditions for each dependent variable in the co- tion temperature led to the dissipation of CO2 through the
gasification of SD and WP with CL were found to be the tem- Boudouard reaction, thereby increasing the yield of CO during
perature for H2/CO ratio in syngas and the equivalence ratio in co-gasification [15]. Hence, it is expected that the concentra-
HHVsyngas. A further comprehensive study on the interaction tion of H2 and CO in syngas would increase during the
factor with regression coefficients will be elaborated in the experiment. Based on the properties of CL/WP, it was notice-
following sections. able that blends of CL and WP possess higher VM, which
makes it a highly volatile content matter, eventually
Effect of operating variables on the H2/CO ratio in the enhancing the production of combustible gases required to
syngas lessen the process temperature and hence, lead to a decrease
in H2 concentration [32]. Whereas in this study, co-gasification
Fig. 5(aef) presents the effects of the three operating variables of CL/WP eventually resulted in a high H2/CO ratio in the
and its interactions with the H2/CO ratio in the syngas for the syngas with highly volatile matter. This is supported by Her-
co-gasification of CL/SD and CL/WP, respectively. The relative nandez et al. [33], claiming that concurrently raising the
importance of these variables are shown in Tables 4 and 5 The biomass content, and temperature in co-gasification leads to a
minimum and maximum values for the H2/CO ratio in syngas higher production of hydrogen. In the case of the co-
for CL/SD were 0.3796 and 1.5837, respectively. In contrast, the gasification of CL/WP, the maximum H2/CO ratio in the syn-
minimum and maximum values for the H2/CO ratio in syngas gas was 25% of the coal blending ratio with the gasification
for CL/WP were 0.7305 and 1.6910, respectively. The influence temperature at 850  C. Considering the raw and treated
of the operating variable for both co-gasifications on the H2/ (pelletized) sawdust, the WP indicates that much more effec-
CO ratio in the syngas was in the order of Temp.>ER >Coal. tive gasification may be due to its physical aspects, such as the
The plot shows that the rise of the H2/CO ratio in syngas by large amount of pores between the SD, which makes it diffi-
increasing the gasification temperature is noticeable at a cult for the heat to react efficiently by moving rapidly from the
higher temperature of 850  C. Raising the temperature pro- accumulation surface to its interior.
vides more energy, which is sufficient for breaking the For the operating factors of the equivalence ratio, both co-
macromolecular structure of the biomass comprising poly- gasifications possess similar results, whereby an increase in
mers of cellulose, hemicellulose and lignin, thus, acting as a the equivalence ratio from 0.20 to 0.30 causes an increase in
catalyst for improving co-gasification. Increasing the tem- CL/SD and CL/WP by 8% and 29%, respectively. The increment
perature also leads to a decrease in CO2 and heavier hydro- of H2/CO was due to the increase in the equivalence ratio
carbon contents, eventually improving the H2 formation. occurring at a higher temperature that resulted in higher
Moreover, the formation of hydrocarbons and tar were con- feedstock conversion and produced higher fuel quality [34].
verted into CO and H2 by reforming reactions. Hence, it is This might be due to the equivalence ratio that is related to
apparent that temperature has a significant effect on the airflow rate and residence time, which is controlled by the
production of the H2/CO ratio in syngas for both co- degree of combustion that depends on the varying amounts of
gasifications. When monitoring the temperature range from O2 supply and leads to a significant effect on the gasification
650  C to 850  C for the co-gasification of CL/SD and CL/WP, the temperature. This leads to a decrease in the energy content of

Fig. 6 e Predicted versus actual values of (a) co-gasification of CL/SD (b) co-gasification of CL/WP on the H2/CO ratio in the
syngas.

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
10 international journal of hydrogen energy xxx (xxxx) xxx

the gas produced because a part of the feedstock’s energy is by the low fixed carbon content of the CL/WP blends that
depleted during the combustion process in the gasification reduced CO production due to its consumption in the water
mechanism. gas shift reaction [35] resulting in the decrease of the H2/CO
Moreover, it can be seen in CL/SD that increasing the coal ratio as the amount of coal increases. This result was similar
blending ratio from 25% to 75% increases the H2/CO ratio in to Brar et al. [36], who revealed that by increasing the amount
the syngas by 12%. This is in contrast with CL/WP, in which of coal in the hardwood pellet, the H2 and CO composition of
the value of the H2/CO ratio in the syngas had decreased by the product gas was reduced. In addition, it can be explained
12% as the coal blending ratio increased. This can be explained that the presence of the oxygen constituent in the biomass

Fig. 7 e 3-Dimensional response surface plot representing combined effects for each (aec) co-gasification of CL/SD (def) and
co-gasification of CL/WP on HHVsyngas.

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
international journal of hydrogen energy xxx (xxxx) xxx 11

Fig. 8 e Predicted versus actual value of (a) co-gasification CL/SD (b) co-gasification CL/WP on HHVsyngas.

Predicted versus actual values of the co-gasification of CL/


Table 6 e Optimum process variables, predicted mode
SD and CL/WP are presented in Fig. 6(a) and (b), respectively.
and confirmation values of response.
The predicted and actual response values of both the co-
Parameters Limits
gasifications are shown in the quadratic regression model.
A: Coal blending ratio 25e75% CL/WP shows a higher R2 at 0.98, whereas the R2 in CL/SD is at
B: Temperature 650e850  C 0.89. The maximum value for the H2/CO ratio in CL/SD’s syn-
C: Equivalence ratio 0.20e0.30
gas was achieved with a coal blending ratio, gasification
H2/CO ratio in the syngas maximize
HHVsyngas maximize
temperature and equivalence ratio of 75%, 850  C and 0.30,
respectively. This is in contrast to CL/WP, where the
maximum values for the H2/CO ratio in the syngas comprised
25% of the coal blending ratio, gasification temperature of
results in a very high production of CO [13], eventually 850  C and 0.30 of the equivalence ratio. Meanwhile, the
reducing the H2 composition of the gaseous product leading to minimum H2/CO ratio in the syngas for both co-gasifications
a decreased value of H2/CO ratio in the syngas. of CL/SD and CL/WP was at (25%-650 C-0.30) and (50%-750

Fig. 9 e Contour plots showing coal blending ratio and temperature for each output variable at optimum condition for co-
gasification for (a) CL/SD (b) CL/WP with ER at 0.30.

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
12 international journal of hydrogen energy xxx (xxxx) xxx

Table 7 e Optimum process variables, model prediction and confirmation values of responses.
Biomass Coal blending Temp. ( C) ER Model predicted value Confirmation run value Desirability
ratio (%)
H2/CO HHVsyngas H2/CO HHVsyngas
SD 75 850 0.30 1.488 5.535 1.58 ± 0.55 5.2683 ± 1.04 0.855
WP 55 816 0.30 1.385 5.333 1.28 ± 0.31 4.8705 ± 0.65 0.762


C-0.15), respectively. This shows that the CL/SD and CL/WP predicted and actual response values of co-gasification follow
values were placed adjacently along the linear straight line the quadratic regression model. The R2 for CL/SD and CL/WP
and this denotes an agreeable regression model. Generally, were calculated at 0.94 and 0.97, respectively. The maximum
increasing the temperature and equivalence ratio results in a value of the HHVsyngas for CL/SD are coal blending ratio,
high amount of H2/CO ratio in the syngas due to the co- gasification temperature and equivalence ratio with values at
gasification of SD/CL. However, for the coal blending ratio, 75%, 850  C and 0.20, respectively. Despite this, the maximum
CL/SD favours higher amounts of coal for increasing the H2/CO value of HHVsyngas for CL was at 50% of coal blending ratio, a
ratio. Whereas, CL/WP favours a lesser amount of coal to gasification temperature of 750  C and 0.25 of equivalence
produce the highest amount of H2/CO ratio in the syngas. ratio. Meanwhile, the minimum H2/CO ratio in the syngas for
the co-gasification of CL/SD and CL/WP was at (75% - 650  C -
Effect of operating variables on higher heating value of 0.30) and (50% - 750  C - 0.35), respectively. The observed
syngas (HHVsyngas) values for both CL/SD and CL/WP correspond to the predicted
value of HHVsyngas.
The effect of three operating variables on HHVsyngas for the co-
gasification of CL/SD and CL/WP are shown in Fig. 7(aef) in the Process optimization and model validation
form of 3-dimensional response surface plots. Tables 3 and 4
show that both the gasification temperature and equivalence The optimization of the coal blending ratio, gasification tem-
ratio mainly affect the HHVsyngas for both SD and WP co- perature, and equivalence ratio for maximum H2/CO ratio in
gasified with CL. The maximum and minimum values of the the syngas, HHVsyngas and Ysyngas for both co-gasifications was
HHVsyngas for CL/SD are 6.0724 MJ/Nm3 and 3.7768 MJ/Nm3, performed by applying the numerical optimization method.
respectively. Complementary to this, the maximum and Table 6 presents the optimization process with a desired range
minimum values of the HHVsyngas for CL/WP were 6.0160 MJ/ of variables and response output. The contour plots showing
Nm3 and 3.4323 MJ/Nm3, respectively. As the gasification optimum input variables for maximum output variables in the
temperature increased from 650  C to 850  C, both of the CL/SD co-gasification of SD and WP with coal are shown in Fig. 9.
and CL/WP’s HHVsyngas increased by 17% and 15%, respec- Confirmation based on the optimized value were conducted in
tively. Fig. 7 shows that the influence of the operating variable triplicates. Table 7 shows the average value for each of the H2/
for both co-gasifications on HHVsyngas was in a similar order as CO and HHVsyngas with standard deviation. A comparison
the H2/CO ratio in the syngas. This study confirms that an between the experimental and predicted results was calcu-
increase in the HHVsyngas is associated with higher gasification lated and shows that the error is less than 7%. It can be
temperatures that cause endothermic gasification reactions, concluded that the developed model can accurately predict
resulting in more heat loss in the system, hence, improving the output variables.
the gasification process during syngas production [37].
Inversely, the HHVsyngas for the co-gasification of CL/SD
and CL/WP had decreased by about 7% with the increase of ER. Conclusions
As ER is related to the airflow rate, a high ER contributes to a
higher airflow rate leading to lower heating values for syngas Extensive and comparative statistical analyses between the
and eventually reducing the efficiency of the gasification co-gasification of CL/SD and CL/WP on individual and com-
process [3,37]. These factors contribute to the reaction’s bined effects of co-gasification operating variables (coal
shorter residence time as the airflow rate increases during the blending ratio, temperature, and equivalence ratio) at
gasification process [29,38]. different process parameters of H2/CO and ratio and heating
Moreover, the term of the coal blending ratio saw a 4% and value of the syngas (HHVsyngas) were performed by applying
7% increase in the HHVsyngas as the amount of the coal response surface methodology (RSM) from a series of gasifi-
increased in the co-gasification with SD and WP, respectively. cation experiments. These experiments were carried out in
This can be attributed to the gasification temperature and coal the external heated fixed-bed downdraft using air as an
blending ratio, which improves the formation of H2 and CO oxidizing agent. The gasification temperature was found to be
that eventually increases the HHVsyngas [39,40]. Subsequently, a prominent variable for the co-gasification between SD and
addition of coal in co-gasification led to a slight increase in WP. Increasing the gasification temperature resulted in an
methane (CH4) production, eventually increasing the amount increase of all the response variables (H2/CO ratio in the syn-
of HHVsyngas [41]. gas and HHVsyngas). Moreover, an increase in the ER in the
Fig. 8(a) and (b) present the predicted versus actual values gasification experiment resulted in an increase in the airflow
of co-gasification of CL/SD and CL/WP, respectively. The rate, eventually minimising the residence time and in turn,

Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
international journal of hydrogen energy xxx (xxxx) xxx 13

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response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029
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Please cite this article as: Mansur FZ et al., Co-gasification between coal/sawdust and coal/wood pellet: A parametric study using
response surface methodology, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.04.029

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